Pressure-driven density match nucleates metastable r8 phases from amorphous Si and Ge

Haberl, Bianca; Guthrie, Malcolm; Jung, Gang Seob; Aji, Leonardus Bimo Bayu; Molaison, Jamie J.; Shen, Guoyin; Irle, Stephan; Bradby, Jodie E.

doi:10.1016/j.mattod.2025.08.002

Pressure-driven density match nucleates metastable r8 phases from amorphous Si and Ge

Journal Article · Mon Aug 18 04:00:00 EDT 2025 · Materials Today

DOI:https://doi.org/10.1016/j.mattod.2025.08.002· OSTI ID:3002502

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). High Pressure Collaborative Access Team (HPCAT)
Australian National Univ., Canberra, ACT (Australia)

The pressure–temperature phase behavior of covalent disordered solids such as amorphous silicon and germanium is complex. Questions remain on possible glass transitions, on polyamorphism via amorphous–amorphous transitions, on connections with liquid–liquid transitions, on structure-behavior relationships, and on their potential as precursor for novel methods for material discovery. Here we demonstrate experimentally the nucleation of a metastable, four-fold coordinated rhombohedral r8 phase from pure amorphous silicon and germanium upon room temperature compression at pressures below 10 GPa. Accompanying theory reveals a strong pressure-driven distortion of the bond angle transforming the starting tetrahedral low-density amorphous network to a distorted four-fold coordinated medium-density state. This state is of lower density than metallic high-density networks, resembles the crystalline r8 phase and initiates its nucleation. Our finding shows that polyamorphism is not the only possible transformation mode for these amorphous solids and that instead nucleation of interesting functional phases at potentially useful pressures is possible. Such novel access modes to metastable structures are critical for future exploitability and could be useful for other tetrahedral materials including carbon, where the related (bc8) post-diamond phase remains elusive. Our observed density match between an amorphous and a metastable crystalline phase clearly allows for a new phase transition pathway, while corresponding theory demonstrates how carefully validated atomistic simulations can guide prediction, discovery and synthesis of novel material structures.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Australian Research Council (ARC); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 3002502

Journal Information:: Materials Today, Journal Name: Materials Today Vol. 89; ISSN 1369-7021

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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